具有16-连接的3D共价有机框架用于光催化C(sp3-C(sp2) 交叉合
Meng Lu1, Shuai-Bing Zhang2, Run-Han Li1
1Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization, School of Chemistry, South China Normal University, Guangzhou 510006, P.R. China.
Journal of the American Chemical Society
|September 4, 2024
概括
研究人员为共价有机框架 (COF) 开发了新的16个连接构件,使得3D COF具有前所未有的连接性. 这些先进的COF在催化应用中表现有前途.
科学领域:
- 材料科学
- 超分子化学
- 催化剂
背景情况:
- 在3D共价有机框架 (COF) 中,构成块的价值在历史上被限制在最大12.
- 开发具有更高连接性的COF构件是材料设计中的一个重大挑战.
- 现有的COF结构往往缺乏先进应用的复杂性.
研究的目的:
- 引入一个等级扩展策略,用于合成16个连接的3DCOF构件.
- 使用这些高连接性单元构建新的3D COF.
- 探索这些新型COF的催化潜力,特别是在交叉合反应中.
主要方法:
- 采用了[16 + 2]的施工策略,将基于碳二烯的16连接结构块 (CzTPN) 与线性米连接器 (BD或Bpy) 凝结在一起.
- 合成了两个不同的3DCOF,CzBDCOF和CzBpyCOF.
- 在CzBpy COF上进行 (Ni) 化,以产生用于催化研究的Ni@CzBpy COF.
主要成果:
- 16个连接的构造块的成功合成,并将它们纳入具有sqc拓的3DCOF.
- Ni@CzBpy COF在光反/Ni双催化C ((sp3) -C ((sp2) 交叉合中表现出高性能,达到高达98%的转换率和94%的产量.
- 开发的COF代表了迄今为止COF材料中最高的连接性.
结论:
- 这项工作提供了第一个具有16个连接单元的高连接性3DCOF的例子.
- 合成的COF具有很好的催化活性,展示了它们在有机合成中的潜力.
- 这些发现显著扩大了共价有机框架的结构多样性和应用范围.
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